Belay Zeleke Dilnesa - Eawag-Empa Library

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CHAPTER 2 MATERIALS AND METHODS Table 4 Dissolution reaction used for thermodynamic calculation. Phases Reactions log KS0 ref Al-katoite Ca3Al2 (OH)12 → 3Ca 2+ +2Al(OH)4 − + 4OH − -20.56 d Fe-katoite Ca3Fe2 (OH)12 → 3Ca 2+ +2Fe(OH)4 − + 4OH − -25.56 d Si-poor Al-siliceous hydrogarnet Ca3Al2(SiO4)0.41(OH)10.36→ 3Ca 2+ +2AlO2 − + 0.41HSiO3 2− + 3.59OH − + 3.18H2O -25.47 d Si-rich Al-siliceous hydrogarnet Ca3Al2(SiO4)0.84(OH)8.64 → 3Ca 2+ +2AlO2 − + 0.84HSiO3 2− + 3.16OH − + 2.32H2O -26.70 d Si poor Fe-siliceous hydrogarnet Ca3Fe2(SiO4)0.95(OH)8.2 → 3Ca 2+ +2FeO2 − + 0.95HSiO3 2− + 3.05OH − + 2.1H2O -32.75 d Si rich Fe-siliceous hydrogarnet Ca3Fe2(SiO4)1.52(OH)5.92 → 3Ca 2+ +2FeO2 − + 1.52HSiO3 2− + 2.48OH − + 0.96H2O -34.68 d Al-ettringite Ca6Al2(SO4)3(OH)12·26H2O → 6Ca 2+ +2Al(OH)4 − + 3SO4 2− +4OH − +26H2O -44.90 a, c Fe-ettringite Ca6Fe2(SO4)3(OH)12·26H2O → 6Ca 2+ +2Fe(OH)4 − + 3SO4 2− +4OH − +26H2O -44.00 a, b Al- hydroxy AFm Ca4Al2(OH)12·7H2O → 4Ca 2+ +2Al(OH)4 − + 6OH − +6H2O -25.40. a Fe- hydroxy AFm Ca4Fe2(OH)12·7H2O → 4Ca 2+ +2Fe(OH)4 − + 6OH − +6H2O -30.64 d Al-monosulfate Ca4Al2(SO4)(OH)12·6H2O → 4Ca 2+ +2Al(OH)4 − + SO4 2− +4OH − +6H2O -29.26 a, c Fe-monosulfate Ca4Fe2(SO4)(OH)12·6H2O → 4Ca 2+ +2Fe(OH)4 − + SO4 2− +4OH − +6H2O -31.57 d Al-monocarbonate Ca4Al2(CO3)(OH)12·5H2O → 4Ca 2+ +2Al(OH)4 − + CO3 2− +4OH − + 5H2O -31.47 a, c Fe-monocarbonate Ca4Fe2(CO3)(OH)12·6H2O → 4Ca 2+ +2Fe(OH)4 − + CO3 2− +4OH − + 6H2O -34.59 d Al-hemicarbonate Ca4Al2(CO3)0.5(OH)12·6H2O → 4Ca 2+ +2Al(OH)4 − + 0.5CO3 2− +5OH − + 5.5H2O -29.13 a, c Fe-hemicarbonate Ca4Fe2(CO3)0.5(OH)12·4H2O → 4Ca 2+ +2Fe(OH)4 − + 0.5CO3 2− +5OH − + 3.5H2O -30.83 d Al-Friedel’s salt Ca4Al2(Cl2)(OH)12·4H2O → 4Ca 2+ +2Al(OH)4 − + 2Cl − +4OH − + 4H2O -27.69 f Fe-Friedel’s salt Ca4Fe2(Cl2)(OH)12·4H2O → 4Ca 2+ +2Fe(OH)4 − + 2Cl − +4OH − + 4H2O -28.62 d Fe(OH)3 (am.) Fe(OH)3 + OH - → Fe(OH)4 - -2.60 e Fe(OH)3 (microcr.) Fe(OH)3+ OH - → Fe(OH)4 - -4.10 d Al(OH)3 (am.) Al(OH)3+ OH - → Al(OH)4 - 0.24 a Gibbsite Al(OH)3+ OH - → Al(OH)4 - -1.24 e Gypsum CaSO4 2H2O → Ca 2+ + SO4 2- + 2H2O -4.58 e Portlandite Ca(OH)2 → Ca 2+ + 2OH - -5.2 d Calcite CaCO3 →Ca 2+ + HCO3 − 1.85 e (a ) Lothenbach et al [3], (b) Möschner et al [15], (c) Matschei. et al [52], (d) this study (e) GEMS/PSI TDB [45, 53]. (f) Balonis et al [54] 29
CHAPTER 2 MATERIALS AND METHODS Table 5 Thermodynamic data at standard conditions (298 K, 1 atm) used for the calculation of the liquid phase compositions and for computation of thermodynamic parameters for the synthesized solids. fG° fH° S 0 C 0 p 1 a0 a1 a2 a3 V 0 Ref. Phase [kJ/mol] [kJ/mol] [J/K/mol] [J/mol/K] [J/(mol.K)] [J/(mol.K 2 )] [J K/mol] [J/(mol.K 0.5 )] [cm3/mol] Al-katoite -5008.5 -5535 432 459 292 0.5610 150 d Fe-katoite -4118.6 -4724 165 485 275 0.0627 0 155 d Si-poor Al-siliceous hydrogarnet -5193.5 -5717 342 441 198 0.5967 -9.98E+05 1312 151 d Si-rich Al-siliceous hydrogarnet -5365.2 -5867 310 422 100 0.6342 -2.05E+06 2688 142 d Si-poor Fe-siliceous hydrogarnet -4523.5 -4854 855 612 582 0.6094 2.02E+06 -3040 156 d Si-rich Fe-siliceous hydrogarnet -4752.8 -5044 847 688 766 0.5988 2.29E+06 -4864 161 d Al-ettringite -15205.9 -17535 1900 2174 1939 0.7890 0 0 707 a Fe-ettringite -14282 -16600 1937 2200 1922 0.8550 2.02E+06 0 717 a, b Al-hydroxy AFm -7326.6 -8300 708 930 711 1.0470 0 -1600 274 b Fe-hydroxy AFm -6438 -7431 640 956 694 1.1134 2.02E+06 -1600 286 d Al-monosulfate -7778.5 -8750 821 942 594 1.1680 0 0 309 a, c Fe-monosulfate -6873.2 -7663 1430 968 577 1.2340 2.02E+06 0 321 d Al-monocarbonate -7337.5 -8250 657 881 618 0.9820 -2.59E+06 0 262 a, c Fe-monocarbonate -6674 -7485 1230 950 612 1.1600 -5.73E+05 0 292 d Al-hemicarbonate -7336 -8270 713 906 664 1.0140 -1.30E+06 -800 285 a, c Fe-hemicarbonate -5952.9 -6581 1270 841 308 1.2014 -9.08E+05 3200 273 d Al-Friedel’s salt -6814.6 -7625 731 829 498 0.8900 -2.03E+06 1503 272 f Fe-Friedel’s salt -5900.1 -6525 1286 855 481 0.9611 -16130 1503 208 d Al(OH)3 (am.) -1143 -1281 70 93 36 0.1910 0 0 32 a Gibbsite -1151 -1289 70 93 36 0.1910 0 0 32 e Fe(OH)3 (am.) -700 -879 88 43 28 0.0520 0 0 34 e Fe(OH)3 (microcr.) -709 -841 88 43 28 0.0520 0 0 34 d Gypsum -1798 -2023 194 186 91 0.3180 0 0 75 e Portlandite -897 -985 83 88 187 -0.0220 0 -1600 33 e Calcite -1129 -1207 93 82 105 0.0220 -2.59E+05 0 37 e CaO -604 -635 40 43 49 0.0040 -6.53E+05 0 17 e Al2O3 -1568 -1662 51 79 115 0.0180 -3.51E+06 0 26 e Fe2O3 -8214 -8214 88 105 98 0.0780 -1.49E+06 0 30 e References: a ) Lothenbach et al. [3], b) Möschner et al. [15], (c) Matschei et al. [52], d) this study, e) Thoenen et al. and Hummel et al. [44, 45], f) Balonis et al. [54] 1 Cp o = a0 + a1T + a2T -2 + a3T -0.5 , Si-poor and Si-rich Al-siliceous hydrogarnet do not form at room temperature 30
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Fe-containing hydrates and their fa
Page 4 and 5: The measured composition of the liq
Page 6 and 7: ZUSAMMENFASSUNG Thermodynamische Mo
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Page 10 and 11: I owe to thank all the laboratory t
Page 12 and 13: Table 19 Compositions of Al/Fe-mono
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Page 16 and 17: Fig. 34 Calculated solubility produ
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Page 20 and 21: Table of Contents TABLE OF CONTENTS
Page 22 and 23: TABLE OF CONTENTS 3. SYNTHETIC FE
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Page 26 and 27: 1 INTRODUCTION CHAPTER 1 INTRODUCTI
Page 28 and 29: CHAPTER 1 INTRODUCTION be formed. T
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Page 40 and 41: 3CaOAl2O3 + 6H2O → 3CaOAl2O36H2O
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CHAPTER 3 SYNTHETIC FE-CONTAINING H
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Intensity [arb. units] Fe-Fr CHAPTE
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CHAPTER 4 FE-CONTAINING HYDRATES IN
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(Al+Fe)/Ca (Al+Fe)/Ca 0.8 0.6 0.4 0
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k 3 (k) CHAPTER 4 FE-CONTAINING HYD
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differentiated relative weight Weig
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Early reaction CHAPTER 4 FE-CONTAIN
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weight loss in % differentiated rel
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5. GENERAL CONCLUSION AND OUTLOOK a
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Speciation of iron(III) in hydrated
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5. GENERAL CONCLUSION AND OUTLOOK
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Techniques XRD X-ray diffraction TG
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APPENDIX APPENDIX Appendix A: Addit
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Intensity (arb. Units) P Fe 2O 3 R
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APPENDIX Appendix B7 XRD patterns o
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REFERENCES REFRENCES [1] H.F.W. Tay
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REFRENCES [29] M. Vespa, R. Dähn,
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REFRENCES [54] M. Balonis, B. Lothe
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REFRENCES [81] H.F.W. Taylor, Cryst
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REFRENCES [107] K. Kyritsis, N. Mel
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REFRENCES [134] M. Wilke, F. Farges
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CURRCULUM VITAE Curriculum Vitae Na
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